CN1013009B - Method for preparing oxide-nuclear fuel sintered matter - Google Patents
Method for preparing oxide-nuclear fuel sintered matterInfo
- Publication number
- CN1013009B CN1013009B CN86102359A CN86102359A CN1013009B CN 1013009 B CN1013009 B CN 1013009B CN 86102359 A CN86102359 A CN 86102359A CN 86102359 A CN86102359 A CN 86102359A CN 1013009 B CN1013009 B CN 1013009B
- Authority
- CN
- China
- Prior art keywords
- material powder
- temperature
- preroast
- crystalline phase
- atmosphere
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired
Links
- 239000003758 nuclear fuel Substances 0.000 title claims abstract description 36
- 238000000034 method Methods 0.000 title claims description 45
- 239000000843 powder Substances 0.000 claims abstract description 78
- 238000005245 sintering Methods 0.000 claims abstract description 48
- 230000001590 oxidative effect Effects 0.000 claims abstract description 13
- 238000010438 heat treatment Methods 0.000 claims abstract description 12
- 239000013078 crystal Substances 0.000 claims abstract description 11
- 239000000203 mixture Substances 0.000 claims abstract description 10
- PSPBAKLTRUOTFX-UHFFFAOYSA-N [O-2].[Pu+4].[U+6].[O-2].[O-2].[O-2].[O-2] Chemical compound [O-2].[Pu+4].[U+6].[O-2].[O-2].[O-2].[O-2] PSPBAKLTRUOTFX-UHFFFAOYSA-N 0.000 claims abstract description 6
- 239000002994 raw material Substances 0.000 claims abstract description 6
- SHZGCJCMOBCMKK-KGJVWPDLSA-N beta-L-fucose Chemical compound C[C@@H]1O[C@H](O)[C@@H](O)[C@H](O)[C@@H]1O SHZGCJCMOBCMKK-KGJVWPDLSA-N 0.000 claims abstract description 4
- 239000000463 material Substances 0.000 claims description 59
- 229910052770 Uranium Inorganic materials 0.000 claims description 31
- 238000001816 cooling Methods 0.000 claims description 24
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 22
- 238000001354 calcination Methods 0.000 claims description 18
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 16
- 239000007789 gas Substances 0.000 claims description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 10
- 229910052757 nitrogen Inorganic materials 0.000 claims description 10
- 239000001301 oxygen Substances 0.000 claims description 10
- 229910052760 oxygen Inorganic materials 0.000 claims description 10
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 8
- 239000001569 carbon dioxide Substances 0.000 claims description 8
- 241000030614 Urania Species 0.000 claims description 7
- FCTBKIHDJGHPPO-UHFFFAOYSA-N uranium dioxide Inorganic materials O=[U]=O FCTBKIHDJGHPPO-UHFFFAOYSA-N 0.000 claims description 7
- 239000002826 coolant Substances 0.000 claims description 5
- 238000005243 fluidization Methods 0.000 claims description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 4
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 claims description 2
- 229910052778 Plutonium Inorganic materials 0.000 claims 10
- 229910052799 carbon Inorganic materials 0.000 claims 3
- WZECUPJJEIXUKY-UHFFFAOYSA-N [O-2].[O-2].[O-2].[U+6] Chemical compound [O-2].[O-2].[O-2].[U+6] WZECUPJJEIXUKY-UHFFFAOYSA-N 0.000 abstract 2
- 229910000439 uranium oxide Inorganic materials 0.000 abstract 2
- 229910052698 phosphorus Inorganic materials 0.000 description 17
- 230000008569 process Effects 0.000 description 10
- 239000000446 fuel Substances 0.000 description 5
- 230000004992 fission Effects 0.000 description 4
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 description 4
- 239000011812 mixed powder Substances 0.000 description 3
- 239000000654 additive Substances 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 239000003595 mist Substances 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 238000007669 thermal treatment Methods 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000002050 diffraction method Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- PNDPGZBMCMUPRI-UHFFFAOYSA-N iodine Chemical compound II PNDPGZBMCMUPRI-UHFFFAOYSA-N 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 238000005649 metathesis reaction Methods 0.000 description 1
- 238000001683 neutron diffraction Methods 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C21/00—Apparatus or processes specially adapted to the manufacture of reactors or parts thereof
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
- G21C3/42—Selection of substances for use as reactor fuel
- G21C3/58—Solid reactor fuel Pellets made of fissile material
- G21C3/62—Ceramic fuel
- G21C3/623—Oxide fuels
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
Landscapes
- Engineering & Computer Science (AREA)
- Physics & Mathematics (AREA)
- Plasma & Fusion (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Chemical & Material Sciences (AREA)
- Ceramic Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
- Compositions Of Oxide Ceramics (AREA)
- Glass Compositions (AREA)
Abstract
氧化铀原料粉末，氧化铀和氧化钚原料粉末的混合物或铀钚氧化物混晶原料粉末的压块在1000℃至1400℃的烧结温度下，先在氧化性气氛中，接着在还原性气氛中进行热处理以制备氧化物核燃料烧结体。为了易于调节核燃料烧结体微观结构中均匀分布的粗晶的浓度，原料粉末和/或压块先在低于烧结温度的条件下预焙烧以生成U4O9或(U，PU)4O9晶相，然后在保持这些晶相不变的前提下先冷却到起始温度，接着在同样前提下再加热到烧结温度。Uranium oxide raw material powder, a mixture of uranium oxide and plutonium oxide raw material powder, or a compact of uranium-plutonium oxide mixed crystal raw material powder at a sintering temperature of 1000°C to 1400°C, first in an oxidizing atmosphere and then in a reducing atmosphere Heat treatment is performed to prepare an oxide nuclear fuel sintered body. In order to easily adjust the concentration of uniformly distributed coarse crystals in the microstructure of nuclear fuel sintered bodies, raw material powders and/or compacts are pre-calcined at a temperature lower than the sintering temperature to generate U 4 O 9 or (U,PU) 4 O 9 crystalline phase, then cooled to the initial temperature while maintaining these crystalline phases, and then reheated to the sintering temperature under the same premise.
Description
The composition that the present invention relates to its material powder of method that potpourri or uranium-plutonium oxide mixed crystal material powder with urania material powder, urania-plutonium oxide material powder prepare oxide-nuclear fuel sintered matter can be UO
2+x, P
UO
2+xOr (U, P
U) O
2+x
European patent registration number 0078428 has been delivered a method of the same type.Owing to generated the U that can survey scope in crystalline phase in the briquetting
4O
9Or (U, P
U)
4O
9Crystalline phase, so the oxide-nuclear fuel sintered matter that makes according to known procedures has equally distributed coarse grain microstructure, it is stable that the nuclear fuel of this structure is grown under reactor operating temperature.Because any crystal boundary no longer takes place to be moved, so fission product gaseous state or volatile, as nitrogen or iodine, can outwards not overflow owing to crystal boundary moves from the oxide matrix of nuclear fuel, therefore be during when what use in the reactor, can in involucrum, do not form undesirable overvoltage with the made fuel rod of this oxide-nuclear fuel sintered matter.Secondly, need not contain the sinter additives that promotes grain growth in the briquetting, this additive may affect the density of nuclear fuel sintered matter.Briquetting U in known method
4O
9Or (U, P
U)
4O
9Crystalline phase is to generate when being heated to sintering temperature in the atmosphere of oxidisability.In order to generate the U of sufficient amount
4O
9Or (U, P
U)
4O
9Crystalline phase, the method need one period holdup time usually, and briquetting will remain in 400 ℃ to the 600 ℃ oxidizing atmospheres in the scope in this section is warmed up to time of sintering temperature.The length of hold-up time depends on the ratio of oxygen and uranium in urania-material powder, i.e. O/U ratio.For example, typical O/U is than being holdup time under 2.1 a certain temperature of urania-material powder in 400 ℃ to 600 ℃ scopes to be at least 1.5 hours, and briquetting can be converted into U fully like this
4O
9Or (U, P
U)
4O
9Crystalline phase.
In addition, by the oxide-nuclear fuel sintered matter that known method makes, in its micromechanism in the concentration of equally distributed coarse-grain and the sintering temperature-rise period and sintering process in the oxidability that oxidizing atmosphere had relevant.Oxidability is defined by the following relationship formula:
△ G
02=RTlnP
02, R=universal gas constant wherein, T=absolute temperature and P
02The dividing potential drop of oxygen in the=oxidizing atmosphere.
Task of the present invention is to further develop known method, makes it easy to regulate equally distributed coarse-grain concentration in the nuclear fuel sintered matter micromechanism.
In order to solve this task, can adopt following creative method: be about to the urania material powder, urania-plutonium oxide raw material powder mixture, uranium-plutonium oxide mixed crystal material powder briquet, and under 1000 ℃ to 1400 ℃ sintering temperature, earlier in oxidizing atmosphere, then in reducing atmosphere, heat treatment contains in crystalline phase can survey U in the scope
4O
9Or (U, P
U)
4O
9The briquetting of crystalline phase just can be prepared the oxide fuel sintered body.It is characterized in that material powder and/or briquetting are being lower than under the sintering temperature of sintering temperature, then preroast in the oxidizing atmosphere of oxidability is arranged, to generate U
4O
9Or (U, P
U)
4O
9Crystalline phase in the cooling atmosphere of inertia or oxidisability, is keeping U then
4O
9Or (U, P
u)
4O
9Under the constant prerequisite of crystalline phase, be cooled to earlier be lower than the initial temperature of sintering temperature, under same prerequisite, in inertia or oxidisability heating atmosphere, be heated to sintering temperature again.
Thermal treatment and the thermal treatment of briquetting in the sintering process in later stage in the preroast process of material powder or briquetting is irrelevant.Like this, can be with the U in material powder or the briquetting by preroast
4O
9Or (U, P
U)
4O
9The concentration of crystalline phase is adjusted to desirable numerical value very accurately, thereby can correspondingly accurately regulate the concentration by coarse-grain in the prepared oxide-nuclear fuel sintered matter microstructure of sintering.Just can on purpose change its plasticity by the distribution ratio of regulating two kinds of grain sizes in the oxide-nuclear fuel sintered matter.When using by fuel rod that this sintered compact constituted in the reactor, its plasticity is significant for the mechanical interaction of rod and shell.Rise to sintering temperature from initial temperature during the briquetting heating and do not need one period special hold-up time.
Method of the present invention can adopt following method and measure to improve its flexibility and economy.
The preroast of material powder will reach the U that generates at least 20 weight %
4O
9Or (U, P
u)
4O
9Crystalline phase is converted into U fully
4O
9Or (U, P
u)
4O
9Crystalline phase is better.After the material powder of preroast is cooled to initial temperature, can mix mutually with an amount of material powder, mixed proportion is for making U in the mixture
4O
9Or (U, P
u)
4O
9The content of crystalline phase is at least 20 weight %, and material powder also can first briquet, and prebake burns the U that generates at least 20 weight % again
4O
9Or (U, P
u)
4O
9Crystalline phase preferably is converted into these crystalline phases fully.The atmosphere of material powder and/or briquetting preroast is the oxidizing atmosphere with oxidability, in this atmosphere, except generating U
4O
9Or (U, P
u)
4O
9Outside the crystalline phase, also generate crystalline phase and can survey the interior U of scope
3O
8Or (U, P
u)
3O
8Crystalline phase.Calcination atmosphere is the mixed gas of 1 atmospheric pressure carbon dioxide or nitrogen and oxygen, preferably selects air for use.The initial temperature of roasting is 20 ℃～30 ℃, is that initial temperature is better with the environment temperature.Optional 70～400 ℃ of sintering temperature, the preroast time elects 10 minutes as～6 hours, also optional 70 ℃～200 ℃ of sintering temperature, the preroast time is selected 10 minutes to 2 hours, also optional 200 ℃～400 ℃ of sintering temperature, the preroast time selects 10 minutes～and 30 minutes.
Urania and/or uranium, plutonium oxide mixed crystal material powder also can prepare being higher than under the sintering temperature, and cooling in an inert atmosphere earlier, and then preroast in the oxidisability calcination atmosphere is from reaching ceiling temperature, till reaching lower limit temperature.In cooling atmosphere, be cooled to initial temperature then.The ceiling temperature of preroast is elected 170 ℃～280 ℃ as, and 250 ℃ better, and lower limit temperature is elected 120 ℃～150 ℃ as, and 130 ℃ better.Material powder between the upper and lower limit temperature during preroast initial cooling velocity be 10 ℃/assign to 20 ℃/minute, stopping cooling velocity is 0.1 ℃/minute.In the calcination atmosphere of reactor, be fluidization during the material powder roasting, and by being cooled to lower limit temperature with the heat exchange of reacting the cooling agent (preferably selecting water) in the chuck from ceiling temperature.
The initial temperature of sending into the cooling medium of reactor jacket is 20 ℃ to 30 ℃, preferably environment temperature.Cooling atmosphere can adopt nitrogen, rare gas, and the mist of the mist of carbon dioxide and oxygen or nitrogen and oxygen selects air better.Pressure is 1 atmospheric pressure.Heating atmosphere adopts rare gas, and nitrogen and/or carbon dioxide, pressure are 1～1.5 crust.
In 1000 ℃ to 1400 ℃ sintering range, finish the heat treated oxidizing atmosphere of briquetting, can use the potpourri of carbon dioxide or carbon dioxide and oxygen, also available air, the pressure of oxidizing atmosphere is generally an atmospheric pressure.Next step reducing atmosphere of heat-treating in 1000 ℃ to 1400 ℃ temperature ranges can be used hydrogen, or the potpourri of hydrogen and a kind of inert gas (for example nitrogen or rare gas), and its pressure also is an atmospheric pressure.The processing time (sintering time) of briquetting in oxidizing atmosphere is generally 15 minutes to 2 hours in 1000 ℃ to 1400 ℃ sintering range, and the heat treatment time in reducing atmosphere (recovery time) is chosen as 15 minutes to 1 hour usually thereafter.
The U that obtains by preroast in material powder or the briquetting
4O
9Or (U, P
U)
4O
9Crystalline phase and U
3O
8-or (U, P
U)
3O
8The concentration of crystalline phase can (be seen " Solid State Communications " with roentgen's diffractometry method, the 5th volume, the 349-352 page or leaf, 1967) or the neutron diffraction measuring method (see " Le Journal de Physique ", the 25th volume, the 431-439 page or leaf, 1964) lattice paprmeter of measuring this briquetting is determined.
The present invention and advantage thereof can be illustrated in greater detail by following example: all example all adopts the UO that makes by so-called AUC process
2Make material powder.This AUC process is seen and is set forth in " Ge Meilin handbook of inorganic chemistry ", uranium, ancillary volume A3,1981,101 pages to 104 pages.In the material powder of example 1 to 8, its oxygen/uranium, namely the O/U ratio is 2.10, the O/U ratio is 2.0 in the example 9.
In example 1 and 2, material powder is preroast under an atmospheric calcination atmosphere in special roaster, is cooled to 20 ℃ of environment temperatures after the preroast in an atmospheric cooling atmosphere, then briquet.Briquetting is heated to sintering temperature in pressure is the heating atmosphere of 1 bar in sintering furnace, and in oxidizing atmosphere sintering, then in same stove, in reducing atmosphere, reduce, be cooled to again at last environment temperature.Table 1 has provided the process conditions of example 1 and 2, coarse-grain and thin brilliant concentration in crystalline phase concentration that preroast obtains and the oxide-nuclear fuel sintered matter that makes.
The table I
Example 1 example 2
140 ℃ 160 ℃ of sintering temperatures
Roasting time 20 minutes 1 hour
Calcination atmosphere air air
Cooling atmosphere air air
20 weight %, 100 weight % in the material powder of preroast
U
4O
9The concentration of crystalline phase
Heating atmosphere CO
2N
2
Oxidizing atmosphere CO during sintering
2CO
2
1100 ℃ 1100 ℃ of sintering temperatures
Sintering time 1 hour 1 hour
Reducing atmosphere H
2H
2
1100 ℃ 1100 ℃ of reduction temperatures
15 minutes 1 hour recovery time
Oxide nuclear fuel sintering 40% 100%
The concentration of coarse-grain in the body (25 microns)
(continuous table I) example 1 example 2
Oxide nuclear fuel sintering 60% 0%
The concentration of thin brilliant (3-5 micron) in the body
Example 3 and 4 material powder with contain U by the program of example 1 and 2 through what preroast made
4O
9The powder of crystalline phase mixes mutually.The mixed-powder briquet, and make oxide-nuclear fuel sintered matter by the program of example 1 and 2.The table II has provided U in the mixed composition
4O
9The concentration of crystalline phase, coarse-grain and thin brilliant concentration in the share of each mixed composition and the oxide-nuclear fuel sintered matter.
The table II
Example 3 examples 4
Powder 1(crosses 100% 80% through preroast
Material powder) in
U
4O
9The share of crystalline phase
Powder 2(is without preroast 0% 0%
The material powder of crossing) in
U
4O
9The share of crystalline phase
Powder 1 50% 70% in the mixed-powder
Share
Powder 2 50% 30% in the mixed-powder
Share
Oxide nuclear fuel sintering 60% 70%
Coarse-grain in the body (25 microns)
Concentration
Continuous table II example 3 examples 4
Oxide nuclear fuel sintering 40% 30%
Thin brilliant (3-5 in the body
Micron) concentration
Example 5 and 6 material powder elder generation briquet, briquetting is preroast under 1 atmospheric calcination atmosphere in calciner, then in 1 atmospheric cooling atmosphere, be cooled to 20 ℃ of the environment temperatures of initial temperature, then press program further processing in sintering furnace of example 1 and 2.The table III has provided the O/U ratio of briquetting in the example 5 and 6, the process conditions of briquetting preroast, U in the briquetting after the preroast
4O
9Coarse-grain and thin brilliant concentration in the concentration of crystalline phase and the oxide-nuclear fuel sintered matter.
Table III example 5 examples 6
Initial o/u is than 2.12 2.12 in the briquetting
150 ℃ 180 ℃ of sintering temperatures
Roasting time 30 minutes 1 hour 10 minutes
Calcination atmosphere air air
Cooling atmosphere air air
In the briquetting of preroast 20% 100%
U
4O
9The concentration of-crystalline phase
In the oxide-nuclear fuel sintered matter 40% 100%
The concentration of coarse-grain (25 microns)
In the oxide-nuclear fuel sintered matter 60% 0%
The concentration of thin brilliant (3-5 micron)
Can find out to showing III that from the table I coarse-grain and thin brilliant concentration can be adjusted to desirable numerical value in the oxide-nuclear fuel sintered matter in very wide scope.
Example 7 Raw powder in special roaster, preroast under an atmospheric calcination atmosphere, sintering temperature and roasting time are selected by this, namely except generating U
4O
9Crystalline phase also generates U outward
3O
8Crystalline phase.This powder is pressed the program cooling of example 1 and 2 again, briquet, and make oxide-nuclear fuel sintered matter by the method for example 1 and 2.
In the example 8, by the briquetting of material powder compacting, its O/U ratio is 2.12, and preroast under an atmospheric calcination atmosphere in special roaster is except generating U
4O
9Crystalline phase also generates U outward
3O
8Crystalline phase, the program by example 5 and 6 is processed into oxide-nuclear fuel sintered matter with briquetting then.
The table IV has provided the process conditions of material powder or briquetting preroast, U in powder that preroast obtains or briquetting
4O
9Crystalline phase and U
3O
8Coarse-grain and thin brilliant concentration in the concentration of crystalline phase and the oxide-nuclear fuel sintered matter that makes.
The table IV
Example 7 examples 8
150 ℃ 150 ℃ of sintering temperatures
Roasting time 2 hours 2 hours
Calcination atmosphere air air
U
4O
9The concentration of crystalline phase 85% 83%
(in the powder) (in briquetting)
U
3O
8The concentration of crystalline phase 15% 17%
Oxide nuclear fuel sintering 85% 85%
Coarse-grain in the body (25 microns)
Concentration
The continued IV
Example 7 examples 8
Oxide nuclear fuel sintering 15% 15%
Thin brilliant (3-5 in the body
Micron) concentration
The density of the oxide-nuclear fuel sintered matter that makes by example 7 and 8 is 10.26 gram/cubic centimetres, and percentage of open area is 0.85% of its volume.Percentage of open area is the share that can reach the hole on sintered body surface in the sintered body.Thus, ambient gas enters these holes easily on the one hand, and the opposing party aspect gas fission product also is easy to overflow from sintered body.
The density of the sintered body that makes by example 2 is 10.48 gram/cubic centimetres, and percentage of open area is 1.05% of its volume.Compare with this sintered body, the sintered body that makes by example 7 and 8 has lower density and lower percent opening, and its reason is that the sintered body that example 7 and 8 makes is by containing U
3O
8The briquetting processing of crystalline phase.Because percentage of open area is lower, so this sintered body sintered body that the energy force rate example 2 of moisture absorption makes from ambiance is low.In addition, the effusion rate of gas fission product is also low than the sintered body that example 2 makes in nuclear reactor.Therefore, the oxide-nuclear fuel sintered matter that makes by example 7 and 8 was easy to drying before the fuel rod clad of packing into.Moreover they can move the long time in nuclear reactor, and can not form owing to the effusion of gas fission product the pressure that surpasses feasible value in fuel rod.
The material powder that AUC process makes in the example 9 is without reoxidizing, but with temperature be 650 ℃ powder directly from the boiling pool furnace send into reactor, material powder carries out the fluidization cooling with the nitrogen of room temperature (promptly 25 ℃) in reactor, makes it reach a certain ceiling temperature.Reactor is provided with cooling jacket, can feed cooling medium, for example water.After material powder reached ceiling temperature, forming pressure in reactor was that 1.3 crust temperature are 25 ℃ calcination atmosphere, and makes material powder carry out fluidization preroast.Then, material powder is cooled to lower limit temperature by the initial cooling velocity of determining and termination cooling velocity from ceiling temperature.
Reach after the lower limit temperature, be that the nitrogen of 1.3 bar is made the calcination atmosphere in the cooling atmosphere metathesis reactor with pressure again, and make material powder be cooled to initial temperature fully by the water in the continuous replacing reactor jacket, be i.e. 25 ℃ environment temperature.
Be cooled to initial temperature through the material powder of preroast again by example 1 and 2 in through preroast and the such further processing of powder of cooling off.The table V has provided the process conditions of preroast in the reactor, through the U of preroast acquisition
4O
9Coarse-grain and thin brilliant concentration in crystalline phase concentration and the oxide-nuclear fuel sintered matter that makes.
The table V
Example 9
250 ℃ of the ceiling temperatures of material powder preroast
130 ℃ of the lower limit temperatures of material powder preroast
15 ℃/minute of cooling velocity initial values during material powder preroast
0.1 ℃/minute of final value
The calcination atmosphere air
U in the powder of preroast
4O
9100%
The concentration of crystalline phase
Coarse-grain 100% in the oxide-nuclear fuel sintered matter
The concentration of (25 microns)
Thin by brilliant 0% in the oxide-nuclear fuel sintered matter
The concentration of (3-5 micron)
According to example 9, preroast and its preparation process of material powder directly can be linked, that is to say, the preparation process of preroast and material powder can be connected together, thereby save to carrying out the required special heating process of preroast.
Claims (20)
1, with the urania material powder, urania-plutonium oxide raw material powder mixture or uranium-plutonium oxide mixed crystal material powder briquet, and under 1000 ℃ to 1400 ℃ sintering temperature earlier in oxidizing atmosphere, then heat treatment contains in crystalline phase and can survey U in the scope in reducing atmosphere
4O
9Or (U, Pu)
4O
9The briquetting of crystalline phase is characterized in that to prepare the method for oxide-nuclear fuel sintered matter material powder and/or briquetting are being lower than under the sintering temperature of sintering temperature, and preroast in the oxidisability calcination atmosphere with oxidability is to generate U
4O
9Or (U, Pu)
4O
9Crystalline phase in the cooling atmosphere of inertia or oxidisability, is keeping U then
4O
9Or (U, Pu)
4O
9Under the constant prerequisite of crystalline phase, be cooled to earlier be lower than the initial temperature of sintering temperature, then under same prerequisite, in the heating atmosphere of inertia or oxidisability, be heated to again sintering temperature.
According to the method for claim 1, it is characterized in that 2, the preroast material powder should generate the U of 20 weight % at least
4O
9Or (U, Pu)
4O
9Crystalline phase.
According to the method for claim 2, it is characterized in that 3, the preroast material powder is to being converted into U fully
4O
9Or (U, Pu)
4O
9Crystalline phase.
4, according to the method for claim 2, it is characterized in that, be cooled to initial temperature after, through the material powder of preroast and an amount of urania material powder, plutonium oxide material powder and/or uranium-plutonium oxide mixed crystal material powder mix mutually, make U in the mixture of powders
4O
9Or (U, Pu)
4O
9The content of crystalline phase is at least 20 weight %.
According to the method for claim 1, it is characterized in that 5, briquetting is by the urania material powder, plutonium oxide material powder and/or the compacting of uranium-plutonium oxide mixed crystal material powder form, and then preroast should generate the U of 20 weight % at least
4O
9Or (U, Pu)
4O
9Crystalline phase.
According to the method for claim 2, it is characterized in that 6, the preroast briquetting is to being converted into U fully
4O
9Or (U, Pu)
4O
9Crystalline phase.
According to the method for claim 1, it is characterized in that 7, the preroast in having the oxidisability calcination atmosphere of oxidability of material powder and/or briquetting is at this moment except generating U
4O
9Or (U, Pu)
4O
9Outside the crystalline phase, also generate crystalline phase and can survey the interior U of scope
3O
8Or (U, Pu)
3O
8Crystalline phase.
8, according to the method for claim 1, it is characterized in that, utilize the potpourri (preferably selecting air for use) of an atmospheric carbon dioxide or nitrogen and oxygen to make calcination atmosphere.
According to the method for claim 1, it is characterized in that 9, choose 20 ℃ to 30 ℃, particularly environment temperature is made initial temperature.
According to the method for claim 2 to 7, it is characterized in that 10, choose 70 ℃ to 400 ℃ and be sintering temperature, the preroast time is 10 minutes to 6 hours.
According to the method for claim 10, it is characterized in that 11, choose 70 ℃ to 200 ℃ and be sintering temperature, the preroast time is 10 minutes to 2 hours.
According to the method for claim 10, it is characterized in that 12, choose 200 ℃ to 400 ℃ and be sintering temperature, the preroast time is 10 minutes to 30 minutes.
13, according to the method for claim 1, it is characterized in that, urania and/or uranium-plutonium-oxide-mixed crystal material powder prepares being higher than under the sintering temperature, and cooling in an inert atmosphere earlier, then material powder preroast in the oxidisability calcination atmosphere is cooled to initial temperature till reach ceiling temperature and begin to reach lower limit temperature then in cooling atmosphere.
According to the method for claim 13, it is characterized in that 14, ceiling temperature is elected 170 ℃ to 280 ℃ as, lower limit temperature is elected 120 ℃ to 150 ℃ as.
According to the method for claim 14, it is characterized in that 15, ceiling temperature is elected 250 ℃ as, lower limit temperature is elected 130 ℃ as.
16, according to the method for claim 13, it is characterized in that, material powder between ceiling temperature and lower limit temperature during preroast initial cooling velocity be 10 ℃/assign to 20 ℃/minute, stopping cooling velocity is 0.1 ℃/minute.
17, according to the method for claim 13, it is characterized in that, in the calcination atmosphere of reactor, be fluidization during the material powder roasting, and by with reactor jacket in the heat interchange of cooling medium (preferably choosing water) be cooled to lower limit temperature from ceiling temperature.
According to the method for claim 1, it is characterized in that 18, the initial temperature of sending into the cooling medium in the reactor jacket is 20 ℃ to 30 ℃, preferably selects environment temperature for use.
19, according to the method for claim 1, it is characterized in that, utilize nitrogen, rare gas, the potpourri of the potpourri of carbon dioxide and oxygen or nitrogen and oxygen are preferably chosen air and are made cooling atmosphere as cooling atmosphere, and pressure is an atmospheric pressure.
20, according to the method for claim 1, it is characterized in that, utilize rare gas, nitrogen and/or carbon dioxide are as heating atmosphere, and pressure is 1 to 1.5 crust.
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE19853519825 DE3519825A1 (en) | 1985-06-03 | 1985-06-03 | METHOD FOR PRODUCING OXIDIC FUEL INTERMEDIATES |
| DE3519825.7 | 1985-06-03 | ||
| DEP3519825.7 | 1985-06-03 |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN86102359A CN86102359A (en) | 1986-12-03 |
| CN1013009B true CN1013009B (en) | 1991-06-26 |
Family
ID=6272292
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN86102359A Expired CN1013009B (en) | 1985-06-03 | 1986-04-08 | Method for preparing oxide-nuclear fuel sintered matter |
Country Status (9)
| Country | Link |
|---|---|
| US (1) | US4816193A (en) |
| EP (1) | EP0205920B1 (en) |
| JP (1) | JPH0631760B2 (en) |
| KR (1) | KR940004775B1 (en) |
| CN (1) | CN1013009B (en) |
| BR (1) | BR8602530A (en) |
| CA (1) | CA1277130C (en) |
| DE (2) | DE3519825A1 (en) |
| ES (1) | ES8707818A1 (en) |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5932930A (en) * | 1994-06-28 | 1999-08-03 | General Electric Company | Method for fabricating mixed oxide fuel |
| JP3023885U (en) * | 1995-10-18 | 1996-04-30 | 憲次 藤岡 | Walking function recovery trainer |
| FR2949598B1 (en) * | 2009-09-02 | 2013-03-29 | Commissariat Energie Atomique | PROCESS FOR PREPARING A POROUS NUCLEAR FUEL BASED ON AT LEAST ONE MINOR ACTINIDE |
Family Cites Families (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4052330A (en) * | 1975-03-20 | 1977-10-04 | Gen Electric | Sintering uranium oxide using a preheating step |
| DE2855166C2 (en) * | 1978-12-20 | 1982-05-27 | Kraftwerk Union AG, 4330 Mülheim | Process for the production of oxidic nuclear fuel bodies |
| DE2939415C2 (en) * | 1979-09-28 | 1981-11-26 | Kraftwerk Union AG, 4330 Mülheim | Process for the production of high-density oxidic nuclear fuel bodies |
| DE3142447C1 (en) * | 1981-10-26 | 1983-04-14 | Kraftwerk Union AG, 4330 Mülheim | Process for the production of oxidic nuclear fuel sintered bodies |
-
1985
- 1985-06-03 DE DE19853519825 patent/DE3519825A1/en not_active Withdrawn
-
1986
- 1986-04-08 CN CN86102359A patent/CN1013009B/en not_active Expired
- 1986-05-20 DE DE8686106828T patent/DE3663410D1/en not_active Expired
- 1986-05-20 EP EP86106828A patent/EP0205920B1/en not_active Expired
- 1986-05-29 JP JP61124597A patent/JPH0631760B2/en not_active Expired - Lifetime
- 1986-05-30 CA CA000510389A patent/CA1277130C/en not_active Expired - Fee Related
- 1986-06-02 BR BR8602530A patent/BR8602530A/en unknown
- 1986-06-03 ES ES555663A patent/ES8707818A1/en not_active Expired
- 1986-06-03 KR KR1019860004400A patent/KR940004775B1/en not_active Expired - Lifetime
-
1987
- 1987-09-18 US US07/099,687 patent/US4816193A/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| US4816193A (en) | 1989-03-28 |
| CN86102359A (en) | 1986-12-03 |
| EP0205920B1 (en) | 1989-05-17 |
| KR940004775B1 (en) | 1994-05-28 |
| EP0205920A1 (en) | 1986-12-30 |
| BR8602530A (en) | 1987-02-03 |
| ES8707818A1 (en) | 1987-08-16 |
| JPH0631760B2 (en) | 1994-04-27 |
| DE3663410D1 (en) | 1989-06-22 |
| CA1277130C (en) | 1990-12-04 |
| JPS61278789A (en) | 1986-12-09 |
| ES555663A0 (en) | 1987-08-16 |
| KR870000718A (en) | 1987-02-20 |
| DE3519825A1 (en) | 1986-12-04 |
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